Bioorganometallic Chemistry of Enzyme Active Sites with Focus on Hydrogenase

以氢化酶为中心的酶活性位点的生物有机金属化学

• 批准号: 0910679
• 负责人: Marcetta Darensbourg
• 金额: $ 81万
• 依托单位: Texas A&M Research Foundation
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2009
• 资助国家: 美国
• 起止时间: 2009-08-15 至 2013-07-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=0910679&HistoricalAwards=false
• 关键词: Bioorganometallic; Chemistry; Enzyme; Active; Sites

The Research award in the Inorganic, Bioinorganic and Organometallic Chemisry program supports work by Professor Marcetta Darensbourg at the Texas A&M University in College Station, TX, to carry out fundamental studies on small molecule models of enzyme active sites responsible for controlling hydrogen metabolism in nature. In this research, synthetic analogues of the unique metal-organic fragments found in hydrogenase enzymes are prepared and assayed for their ability to mimic the hydrogen-producing and hydrogen-consuming catalysis found in organisms that subsist on a micro-hydrogen economy. The atom-atom connections, the geometrical structure, and spectroscopic footprints of these natural catalysts are reproduced in the small molecules. The intricate and facilitating role of the surrounding protein matrix is approached by imbedding the new molecules in polymer beads and cyclodextrins. By this approach we develop understanding of the way Nature has engineered hydrogen processing ability into base metal constructs of iron and nickel, whereas commercial fuel cells must rely on expensive and resource-limited platinum. Students at all levels (graduates and undergraduates) are excited by the chemistry of fuel cells and interest in hydrogen as an energy carrier is high. In the process of opening young minds to the needed research in alternative energy sources and challenges, inspiration from nature leads into the literature of biology, biochemistry, biophysics, as well as synthetic inorganic chemistry. Our culturally diverse research group works as a team in projects to encourage interest in science in grammar school children; undergraduates from historically black colleges and universities and from South Texas, largely Hispanic colleges, join the research group to help in the projects through summer research. A home-run from this work would result in hydrogen processing catalysts feasible enough to serve as a molecular fuel cell electrode, replacing platinum as a fuel cell electrode, and to make energy-efficient fuel cell technology feasible for a broader range of applications.

无机、生物无机和有机金属化学项目的研究奖支持德克萨斯州大学城德克萨斯 A&M 大学 Marcetta Darensbourg 教授的工作，以对负责控制自然界氢代谢的酶活性位点的小分子模型进行基础研究。在这项研究中，制备了氢化酶中独特金属有机片段的合成类似物，并分析了它们模拟以微氢经济为生的生物体内发现的产氢和耗氢催化的能力。这些天然催化剂的原子-原子连接、几何结构和光谱足迹都在小分子中再现。通过将新分子嵌入聚合物珠和环糊精中，可以发挥周围蛋白质基质的复杂和促进作用。通过这种方法，我们加深了对大自然如何将氢处理能力设计到铁和镍的贱金属结构中的方式的理解，而商业燃料电池必须依赖昂贵且资源有限的铂。各个级别的学生（研究生和本科生）都对燃料电池的化学原理感到兴奋，并且对氢作为能源载体的兴趣很高。在让年轻人接受替代能源和挑战所需的研究的过程中，来自大自然的灵感引导到生物学、生物化学、生物物理学以及合成无机化学的文献中。我们的文化多元化研究小组作为一个团队开展项目，以鼓励文法学校儿童对科学的兴趣；来自历史悠久的黑人学院和大学以及来自德克萨斯州南部（主要是西班牙裔学院）的本科生加入研究小组，通过暑期研究为项目提供帮助。这项工作的成功将导致氢处理催化剂足够可行，可以用作分子燃料电池电极，取代铂作为燃料电池电极，并使节能燃料电池技术在更广泛的应用中可行。